Novel combination catalysts based on iron for the substantial synthesis of multi-walled carbon nanotubes by chemical vapor deposition

ABSTRACT

Methods and systems of preparing a catalyst to be used in the synthesis of carbon nanotubes through Chemical Vapor Depositions are disclosed. The method may include a mixture comprising at least one of an iron catalyst source and a catalyst support. In another aspect, a method of synthesizing multi-walled carbon nanotubes using the catalyst is disclosed. The method may include driving a reaction in a CVD furnace and generating at least one multi-walled carbon nanotube through the reaction. The method also includes depositing the catalyst on the CVD furnace and driving a carbon source with a carrier gas to the CVD furnace. The method further includes decomposing the carbon source in the presence of the catalyst under a sufficient gas pressure for a sufficient time to grow at least one multi-walled carbon nanotube.

CLAIM OF PRIORITY

This is a Divisional Application and claims priority to the U.S. Utilityapplication Ser. No. 12/943,024 titled NOVEL COMBINATION CATALYSIS BASEDON IRON FOR THE SUBSTANTIAL SYNTHESIS OF MULTI-WALLED CARBON NANOTUBESBY CHEMICAL VAPOR DEPOSITION filed on Nov. 10, 2010.

FIELD OF TECHNOLOGY

This disclosure relates to the process of Chemical Vapor Deposition(CVD)for synthesizing multi-wall carbon nanotubes (MWCNT). In particular, thedisclosure relates to creating iron-based novel combination catalystsfor use in the substantial synthesis of multi-walled carbon nanotubesbychemical vapor deposition.

BACKGROUND

Cheap, massive production of multi-walled carbon nanotubes is essentialfrom the commercial point of view. Thus, to achieve this goal, cheap rawmaterials are required. Among these materials is the catalyst used forthe synthesis of multi-walled carbon nanotubes.

Multi-walled carbon nanotubes are candidate for the fabrication ofmaterials possessing novel characters due to their high mechanicalstrength. These new materials can be used for coating, plastic, metalalloys, electronic equipments, gas storage, conductive materials,membranes, drug delivery and many other applications. Thus, a wide rangeof companies can benefit from these materials. Petrochemical,pharmaceutical, electronic, just to mention a few. Expensive catalystsmay drive the cost up and may prove to be ineffective in commerciallyproducing multi-walled carbon nanotubes. A cheap efficient method ofproducing multi-walled carbon nanotubes is required.

SUMMARY

Disclosed are a method, an apparatus and/or a system of chemical vapordeposition for synthesizing multi-walled carbon nanotubes.

Disclosed is a catalyst for synthesizing multi-walled carbon nanotubesby chemical vapor deposition comprising of a mixture including any oneof cyclopentadienyliron dicarbonyldimer[(C₅H₅)₂Fe₂(CO)₄], iron nitratenonahydrate[Fe(NO₃)₃.9H₂O], ferrocene (Fe(C₅H₅)₂) and gamma-phase ofalumina (γ-Al₂O₃) to be used as a catalyst support.

The catalyst is prepared by a set of steps comprising, mixing at leastone of iron nitrate nonahydrate[Fe(NO₃)₃.9H₂O], ferrocene[Fe(C₅H₅)₂]andcyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄] on thegamma-phase of alumina (γ-Al₂O₃) to form a mixture; drying the mixture;calcining the mixture under air at least 400° C. to obtain aγ-Al₂O₃-supported iron oxide pre-catalyst; placing the γ-Al₂O₃-supportediron oxide pre-catalyst into a CVD furnace; flushing theγ-Al₂O₃-supported iron oxide pre-catalyst under a hydrogen flow; andgradually raising a temperature of the CVD furnace to at least 650° C.to obtain the catalyst, γ-Al₂O₃-supported iron metal.

The catalyst for synthesizing multi-walled carbon nanotubes by chemicalvapor deposition at least includes the mixture that is deposited on aChemical Vapor Deposition(CVD) furnace to drive a reaction thatgenerates at least one multi-walled carbon nanotube.

The method of synthesizing multi-walled carbon nanotubes, which at leastincludes the following steps of driving a reaction in a Chemical VaporDeposition (CVD) furnace; generating at least one multi-walled carbonnanotube through the reaction in the CVD furnace; depositing a catalyston the CVD furnace, wherein the catalyst is γ-Al₂O₃-supported ironmetal; driving a carbon source with a carrier gas to the CVD furnace;and decomposing the carbon source in the presence of the catalyst, undera sufficient gas pressure for a sufficient time, to grow themulti-walled carbon nanotube at a target temperature.

Further, the system of synthesizing multi-walled carbon nanotubes bychemical vapor deposition comprises a Chemical Vapor Deposition(CVD)furnace to drive a reaction that generates at least one multi-walledcarbon nanotube;a catalyst deposited on the CVD furnace to enhance thereaction that generates the carbon nanotube, wherein the catalyst isγ-Al₂O₃-supported iron metal; a carbon source gas to react with thecatalyst to grow the carbon nanotube in the CVD furnace.

BRIEF DESCRIPTION OF THE DRAWINGS

The embodiments of this invention are illustrated by way of example andnot limitation in the figures of the accompanying drawings, in whichlike references indicate similar elements and in which:

FIG. 1 is a schematic view of a catalyst preparation, according to oneor more embodiments.

FIG. 2 is a schematic view of a method of synthesizing multi-walledcarbon nanotubes, according to one or more embodiments.

FIG. 3 is a process flow diagram detailing the steps involved in amethod of synthesizing multi-walled carbon nanotubes, according to oneor more embodiments.

FIGS. 4-6 are views of nanotubes shown at various resolutions, accordingto one or more embodiments.

FIG. 7A-7I depicts a table illustrating scientific data acquired inmaking multi-walled carbon nanotubes using many variables. The tabledepicts changes in yield depending on variables like the type ofcatalyst used, percentage of components of the catalyst, reactiontemperature, reaction time and others.

Other features of the present embodiments will be apparent from theaccompanying drawings and from the detailed description that follows.

DETAILED DESCRIPTION

Example embodiments, as described below, may be used to provide amethod, a combination, an apparatus and/or a system of catalysts forsubstantial synthesis of multi-walled carbon nanotubes. Although thepresent embodiments have been described with reference to specificexample embodiments, it will be evident that various modifications andchanges may be made to these embodiments without departing from thebroader spirit and scope of the various embodiments.

A novel combination of catalysts based on iron for the substantialsynthesis of multi-walled carbon nanotubes by chemical vapor depositionare disclosed herein. The catalyst is prepared by simple mechanicalmixing of commercially available materials. A simple, cheap set up ofChemical Vapor Deposition (CVD) process is also adopted by using thiscatalyst for the synthesis of massive, high quality multi-walled carbonnanotubes.

FIG. 1 illustrates the catalyst preparation 100 for the substantialsynthesis of multi-walled carbon nanotubes, according to one or moreembodiments. The Iron catalyst 104 is placed on a catalyst support 102to form a mixture. In one or more embodiments, the catalyst support 102may be γ-Al₂O₃. In one or more embodiments, the iron catalyst 104 may bea cyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄] or/and an ironnitrate nonahydrate [Fe(NO₃)₃.9H₂O] or/and a ferrocene (Fe(C₅H₅)₂). Inone embodiment, when the iron catalyst is the iron nitrate nonahydrate[Fe(NO₃)₃.9H₂O], the mixture was dried at 100° C. The mixture was thencalcined at 450° C. for two hours to obtain a γ-Al₂O₃-supported ironoxide pre-catalyst 110. In one embodiment, the γ-Al₂O₃-supported ironoxide pre-catalyst 110 may be placed on a horizontal electric furnace120. In another embodiment, the γ-Al₂O₃-supported iron oxidepre-catalyst 110 may be placed in a ceramic boat and inserted in aceramic tube and then placed in the furnace 120. The furnace containingthe γ-Al₂O₃-supported iron oxide pre-catalyst 110 was then flushed for30 minutes under a hydrogen flow 114 at room temperature. Thetemperature was then gradually raised to 650° C. and was kept at thistemperature for two hours to obtain the γ-Al₂O₃-supported iron metalcatalyst 130.

In another embodiment, the iron catalyst 104 may be thecyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄]. In thisembodiment, the mixture of the catalyst support 102 and thecyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄] was mixed welland dried at 100° C. The mixture was again calcined at 450° C. for twohours to obtain a γ-Al₂O₃-supported iron oxide pre-catalyst 110. Themixture was then placed in the furnace 120, and then flushed for 30minutes under a hydrogen flow 114 at room temperature. The temperaturewas then gradually raised to 650° C. and was kept at this temperaturefor two hours to obtain the γ-Al₂O₃-supported iron metalcatalyst 130.

As shown in FIG. 1, after the reduction step of reducing theγ-Al₂O₃-supported iron oxide pre-catalyst 110 to produceγ-Al₂O₃-supported iron metalcatalyst 130, a carbon source 116 is flushedat a specific flow rate into the furnace 120. In one embodiment, thetemperature of the furnace was rapidly increased at a rate of 20° C./minto 750° C. The carbon source was then decomposed in the presence of theγ-Al₂O₃-supported iron catalyst 130 for one hour at 750° C. to form amulti-walled carbon nanotube 132.

In one or more embodiments, the carbon source may be a mixture of acarbon source gas and an auxiliary carbon source gas. In anotherembodiment, the carbon source may simply be a carbon source gas. In onone of more embodiments, the carbon source gas 116 may be methane,ethylene, ethane, acetylene, propylene or another suitable hydrocarbongas. The auxiliary carbon source gas may be at least one of toluene,hexane, heptane, methanol, Tetrahydrofuran (THF), cyclohexane, benzeneor another solvent.

In one or more embodiments, the weight percentage ofcyclopentadienyliron dicarbonyl dimer [(C₅H₅)₂Fe₂(CO)₄] in relation tothe gamma-phase of alumina (γ-Al₂O₃) ranges from 80% to 100%.

In one or more embodiments, the weight percentage of the iron nitratenonahydrate [Fe(NO₃)₃.9H₂O]in relation to the gamma-phase of alumina(γ-Al₂O₃) ranges from 15% to 60%.

In one or more embodiments, the weight percentage of the ferrocene(Fe(C₅H₅)₂)in relation to the gamma-phase of alumina (γ-Al₂O₃) rangesfrom 80% to 100%.

In one or more embodiments, the percentage by weight of the gamma-phaseof alumina (γ-Al₂O₃)in relation to the iron catalyst ranges from 0% to85%.

FIG. 2 shows a method of synthesizing multi-walled carbon nanotubes byChemical Vapor Deposition 200, according to one or more embodiments. Themethod of synthesizing multi-walled carbon nanotubes by Chemical VaporDeposition 200 may include the steps of driving a reaction in a ChemicalVapor Deposition furnace 120, generating at least one multi-walledcarbon nanotube 132 through the reaction in the furnace 120, depositinga catalyst 130 on the surface of the CVD furnace 120, wherein theγ-Al₂O₃-supported iron metal catalyst 130 is made from a mixture of atleast one of cyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄], aniron nitrate nonahydrate [Fe(NO₃)₃.9H₂O], a ferrocene [Fe(C₅H₅)₂] and agamma-phase of alumina (γ-Al₂O₃), driving a carbon source with a carriergas 208 to the Chemical vapor deposition (CVD) 120 and decomposing thecarbon source in the presence of the catalyst 130, under a sufficientgas pressure for a sufficient time, to grow the multi-walled carbonnanotube at a target temperature. In one or more embodiments, the targettemperature ranges from 450° C. to 1000° C.

In one or more embodiments, the carbon source is any one of acarbon-source-gas 206 and an auxiliary carbon source 204. In one or moreembodiments, wherein the carbon-source-gas 206 is any one of methane,ethane, ethylene, acetylene, propylene or any other suitable hydrocarbongas. In one or more embodiments, the auxiliary carbon source 204 in anyone of toluene, pentane, hexane, heptane, methanol, ethanol,Tetrahydrofuran (THF), cyclopentane, cyclohexane, benzeneorany othersuitable solvent. In one or more embodiments the carrier gas 208 is anyone of hydrogen, argon, nitrogen or any other suitable gas.

FIG. 3, in one or more embodiments shows a process flow diagram thatdepicts a system of synthesizing multi-walled carbon nanotubes bychemical vapor deposition. In step 302, a reaction may be driven in theCVD furnace 120. In step 304, one or more multi-walled carbon nanotubesmay be generated through the reaction in the CVD furnace 120. Further,in step 306, a catalyst may be deposited on the CVD furnace to enhancethe reaction that generates the multi-walled carbon nanotube. In one ormore embodiments, the catalyst is a gamma-phase of alumina(γ-Al₂O₃)supported iron metal catalyst, derived from an iron source. Instep 308, a carbon source gas with a carrier gas may be driven into theCVD furnace 120. In step 310, the carbon source may be decomposed in thepresence of the catalyst 130 in the CVD furnace 120, under a sufficientgas pressure for a sufficient time, to grow the multi-walled carbonnanotube at a target temperature.

In step 312, a pure gas may be driven into the CVD furnace 120 todisplace a quantity of air in the CVD furnace. In step 314, a flow ofHydrogen may be driven into the CVD furnace 120 to displace the puregas. Further, in step 316, the multi-walled carbon nanometer in areaction time ranging from 15 minutes to 120 minutes.

In one or more embodiments, the precatalyst is a mixture of any one of acyclopentadienyliron dicarbonyl dimer[(C₅H₅)₂Fe₂(CO)₄], an iron nitratenonahydrate[Fe(NO₃)₃.9H₂O], a ferrocene [Fe(C₅H₅)₂] and a catalystsupport 102. In one or more embodiments, the catalyst support 102 may beγ-Al₂O₃.

In one or more embodiments, the target temperature is between 450° C.and 1000° C. In one or more embodiments, a carrier gas drives the carbonsource gas into the CVD furnace 120.

In an example embodiment, the catalyst support is the commerciallyavailable γ-Al₂O₃, having a particle size of 0.015 μm and a high surfacearea of 220 m²/g. The iron catalyst source was loaded on this support bypulverizing it with a specific amount(refer to column 716 in FIG. 7) ofFe(NO₃)₃.9H₂O. The resultant mixture solid was dried at 100° C. and thencalcined under air at 450° C. for two hours to obtain theγ-Al₂O₃-supported iron oxide pre-catalyst. This pre-catalyst was thenplaced in a ceramic boat, inserted in a ceramic tube (diameter: 45 mm;length:100 mm), located in a horizontal electrical CVD furnace. Thecatalyst was flushed for 30 min under a steady hydrogen flow(refer tocolumn 710 in FIG. 7) at room temperature. The temperature was thengradually raised to 650° C. and this temperature was maintained for twohours for the reduction of iron oxide to iron metal, and hence, theobtainment of γ-Al₂O₃-supported iron catalyst. After this reductionstep, a single-gas component or a mixture of two gases was flushed intothe chamber(refer to column 710 in FIG. 7).The temperature of thefurnace was rapidly increased at a rate of 20° C./min to 750° C. Thesynthesis of multi-walled carbon nanotube was carried out at 750° C. forone hour.

In an alternate embodiment, the catalyst support is the commerciallyavailable γ-Al₂O₃, having a particle size of 0.015 μm and a high surfacearea of 220 m²/g. The iron catalyst source 104 iscyclopentadienylirondicarbonyl dimer,[(C₅H₅)₂Fe₂(CO)₄]. The two solids may be crushed, mixedwell, and dried at 100° C. The resultant powder may then be calcined inair at 450° C. for two hours in order to obtain the γ-Al₂O₃-supportediron oxide pre-catalyst. This pre-catalyst was placed in a ceramic boat,inserted in a ceramic tube (diameter: 45 mm; length: 100 mm), located inthe CVD furnace 120. The catalyst may be flushed for 30 min under asteady hydrogen flow (refer to column 710 in FIG. 7) at roomtemperature. For example in Sample 30 in FIG. 7D, hydrogen is flushed inat a rate of 300 ml/min. The temperature may then be gradually raised to650° C. and this temperature was maintained for two hours for thereduction of iron oxide to iron metal, to obtain the γ-Al₂O₃-supportediron catalyst. After this reduction step, a single-gas component or amixture of two gases may be flushed at specific flow rates. For examplein Sample 53 in FIG. 7E, methane gas is flushed in at a rate of 300ml/min. The temperature of the CVD furnace may then be rapidly increasedat a rate of 20° C./min to 750° C. The synthesis of the multi-walledcarbon nanotube may be carried out at 750° C. for one hour.

In one or more of the earlier embodiments, the auxiliary source ofcarbon 204 may be used in order to get better multi-walled carbonnanotube morphology in terms of the diameter and length and maybe evenhigher combustion temperature.

FIGS. 4-6 are views of the multi-walled carbon nanotubes shown atvarious resolutions, according to one or more embodiments. FIG. 4 showsthe generated multi-walled carbon nanotubes at a magnification of 5000.FIG. 5 shows the generated multi-walled carbon nanotubes at amagnification of 50,000 and FIG. 6 shows the generated multi-walledcarbon nanotubes at a magnification of 100,000. In particular, FIG. 6shows nanotubes of various sizes ranging from 7.7 nm to 54.9 nm.

FIGS. 7A-71 is a table that illustrates test results, conducted inproducing multi-walled carbon nanotubes 132. Column 702 describes themorphology of the multi-walled carbon nanotube 132, including a lengthof the multi-walled carbon nanotube 132 in micrometers (tm) and adiameter of the multi-walled carbon nanotube 132 in nanometers (nm). Asper the table, in the set of experiments, the diameter of themulti-walled carbon nanotube ranged from 10-20 nm in 724 as shown inFIG. 7B to 5-80 nm in 726, also in FIG. 7B.The length of themulti-walled carbon nanotube ranged from 20 um to 180 um. Column 704describes a combustion temperature of the reaction to produce themulti-walled carbon nanotube 132. The combustion temperature ranged from572° C. to 700° C. Column 706 describes a weight in grams (g) of thesolvent consumed during the reaction to produce the multi-walled carbonnanotube 132. The solvent is the auxiliary source gas 718. For example,in 728, in FIG. 7A, the auxiliary gas was benzene and 2.99 g wasconsumed to yield 0.737 g of the multi-walled carbon nanotube 132.Column 708 describes the yield in grams (g) of the multi-walled carbonnanotube 132 produced in the reaction. The yield ranged from 0.145 g to8.81 g of the multi-walled carbon nanotube in 730 in FIG. 7I. In theexample embodiment, 730, to obtain 8.81 g of the multi-walled carbonnanotube 132, in 730, 42 g of Toluene was flushed to the CVD furnace;the gas flow rate of C₂H₂ was 291 ml/min; the reaction time was 120minutes; the weight percentage of the support γ-Al₂O₃ when compared tothe iron catalyst 104 was 40%; and the reaction temperature was 750° C.Column 710 describes the gas flow rate. Column 712 describes thereaction time (in minutes) to form the multi-walled carbon nanotubes132. The reaction time in all the example embodiments in the experimentsdescribed in FIGS. 7A-7I was either 60 minutes or 120 minutes. Column714 describes the weight percentage of the components of the supportγ-Al₂O₃ in relation to the iron catalyst source 104. The weightpercentage in the case of the iron nitrate nonahydrate [Fe(NO₃)₃.9H₂O]ranged from 40% to 83.3%. When cyclopentadienyliron dicarbonyl dimer,[(C₅H₅)₂Fe₂(CO)₄] is the iron catalyst 104, the weight percentage rangedfrom 0% to 20%. When Ferrocene was used as the iron catalyst 104, theweight percentage ranged from 0% to 20%.Column 716 describes thecomposition of the catalyst used in the reaction to product themulti-walled carbon nanotubes 132. Column 718 describes the identity ofthe auxiliary carbon source 718, if one was used in the reaction toproduce multi-walled carbon nanotubes 132. Column 720 describes thereaction temperature of the reaction. The reaction temperature rangedfrom 450° C. to 850° C.

While particular embodiments of the present invention have been shownand described, it will be obvious to those skilled in the art that,based upon the teachings herein, changes and modifications may be madewithout departing from this invention and its broader aspects and,therefore, the appended claims are to encompass within their scope allsuch changes and modifications as are within the true spirit and scopeof this invention.

Furthermore, it is to be understood that the invention is solely definedby the appended claims. It will be understood by those within the artthat, in general, terms used herein, and especially in the appendedclaims (e.g., bodies of the appended claims) are generally intended as“open” terms (e.g., the term “including” should be interpreted as“including but not limited to,” the term “having” should be interpretedas “having at least,” the term “includes” should be interpreted as“includes but is not limited to,” etc.).

It will be further understood by those within the art that if a specificnumber of an introduced claim recitation is intended, such an intentwill be explicitly recited in the claim, and in the absence of suchrecitation no such intent is present. For example, as an aid tounderstanding, the following appended claims may contain usage of theintroductory phrases “at least one” and “one or more” to introduce claimrecitations. However, the use of such phrases should not be construed toimply that the introduction of a claim recitation by the indefinitearticles “a” or “an” limits any particular claim containing suchintroduced claim recitation to inventions containing only one suchrecitation, even when the same claim includes the introductory phrases“one or more” or “at least one” and indefinite articles such as “a” or“an” (e.g., “a” and/or “an” should typically be interpreted to mean “atleast one” or “one or more”).

1. A method of synthesizing multi-walled carbon nanotubes, comprising:driving a reaction in a Chemical Vapor Deposition (CVD) furnace;generating at least one multi-walled carbon nanotube through thereaction in the CVD furnace; depositing a catalyst on the CVD furnace,wherein the catalyst is a mixture of at least one of an iron catalystsource and a catalyst support, wherein the iron catalyst source is acyclopentadienyliron dicarbonyl dimer [CpFe(CO)₂]₂, wherein thepercentage by weight of the cyclopentadienyliron dicarbonyl dimer[CpFe(CO)₂]₂ in relation to a gamma phase of alumina (γ-Al₂O₃) rangesfrom 80% to 100%; and wherein the catalyst support is a gamma-phase ofalumina (γ-Al₂O₃); driving a carbon source with a carrier gas to the CVDfurnace; and decomposing the carbon source in the presence of thecatalyst, under a sufficient gas pressure for a sufficient time, to growthe multiwalled carbon nanotube at a target temperature, wherein thecarbon source is at least one of a carbon-source gas and an auxiliarycarbon source.
 2. (canceled)
 3. (canceled)
 4. (canceled)
 5. The methodof claim 1 wherein the percentage by weight of gamma-phase of alumina(γ-Al₂O₃) in relation to the iron catalyst source ranges from 0% to 85%.6. The method of claim 1 wherein the target temperature ranges from 450°C. to 1000° C.
 7. The method of claim 1 wherein the carbon-source-gas isat least one of methane, ethylene, ethane, acetylene and propylene. 8.The method of claim 1 wherein the auxiliary carbon source is at leastone of toluene, hexane, heptane, a methanol, Tetrahydrofuran (THF),cyclohexane and benzene.
 9. The method of claim 1 wherein the carriergas is at least one of hydrogen gas, argon gas, and nitrogen gas. 10.The method of claim 1 further comprising: driving a pure gas into theCVD furnace to displace air in the CVD furnace, wherein the pure gas isat least one of the argon gas and the nitrogen gas.
 11. The method ofclaim 1 further comprising: driving a flow of the hydrogen gas into theCVD to displace the pure gas.
 12. The method of claim 1 furthercomprising: generating the multi-walled carbon nanometer in a reactiontime ranging from 15 minutes to 120 minutes.
 13. The method of claim 1wherein the multi-walled carbon nanometer has a diameter ranging from 5nm to 80 nm.
 14. The method of claim 1 wherein the multi-walled carbonnanotube has a length ranging from 20 um to 180 um.
 15. A method ofsynthesizing multi-walled carbon nanotubes, comprising: generating atleast one multi-walled carbon nanotube through a reaction in a chemicalvapor deposition (CVD) furnace; depositing a catalyst on the CVDfurnace, wherein the catalyst is a mixture of at least one of an ironcatalyst source and a catalyst support, wherein the iron catalyst sourceis a cyclopentadienyliron dicarbonyl dimer [CpFe(CO)₂]₂, and at leastone of an other iron catalyst source, wherein the percentage by weightof the cyclopentadienyliron dicarbonyl dimer [CpFe(CO)₂]₂ in relation toa gamma phase of alumina (γ-Al2O3) ranges from 80% to 100%; and whereinthe catalyst support is a gamma-phase of alumina (γ-Al₂O₃); driving acarbon source with a carrier gas to the CVD furnace; and decomposing thecarbon source in the presence of the catalyst, under a sufficient gaspressure for a sufficient time, to grow the multiwalled carbon nanotubeat a target temperature, wherein the carbon source is at least one of acarbon-source gas and an auxiliary carbon source.
 16. The method ofclaim 15 wherein the other iron catalyst source is at least one of aniron nitrate nanohydrate [Fe(NO₃)₃.9H₂O] and a ferrocene.
 17. (canceled)18. The method of claim 15 wherein the percentage by weight of the ironnitrate nanohydrate [Fe(NO₃)₃.9H₂O]in relation to the gamma-phase ofalumina (γ-Al₂O₃) ranges from 15% to 60%, wherein percentage by weightof the ferrocene in relation to the gamma-phase of alumina (γ-Al₂O₃)ranges from 80% to 100% and wherein the percentage by weight ofgamma-phase of alumina (γ-Al₂O₃)in relation to the iron catalyst sourceranges from 0% to 85%.
 19. A method of synthesizing multi-walled carbonnanotubes, comprising: generating at least one multi-walled carbonnanotube through a reaction in a chemical vapor deposition (CVD)furnace; depositing a catalyst on the CVD furnace, wherein the catalystis a mixture of at least one of an iron catalyst source and a catalystsupport, wherein the iron catalyst source is a cyclopentadienylirondicarbonyl dimer [CpFe(CO)₂]₂, wherein the percentage by weight of thecyclopentadienyliron dicarbonyl dimer [CpFe(CO)₂]₂ in relation to agamma phase of alumina (γ-Al₂O₃) ranges from 80% to 100%; and whereinthe catalyst support is a gamma-phase of alumina (γ-Al2O3); driving acarbon source with a carrier gas to the CVD furnace; and decomposing thecarbon source in the presence of the catalyst, under a sufficient gaspressure for a sufficient time, to grow the multiwalled carbon nanotubeat a target temperature, wherein the carbon source is at least one of acarbon-source gas and an auxiliary carbon source.
 20. The method ofclaim 19 further comprising: preparing the catalyst through a set ofsteps, the set of steps further comprising: mixing thecyclopentadienyliron dicarbonyl dimer [(C5H5)2Fe2(CO)4] with gamma-phaseof alumina (γ-Al2O3) to form a solid mixture; drying the mixture;calcining the mixture under air at least 400° C. to obtain aγ-Al2O3-supported iron oxide pre-catalyst; placing the γ-Al2O3-supportediron oxide pre-catalyst into a CVD furnace; flushing theγ-Al2O3-supported iron oxide pre-catalyst under a hydrogen flow; andgradually raising a temperature of the CVD furnace to at least 650° C.to obtain the catalyst.